Transform method in resonance Raman scattering with quadratic Franck–Condon and Herzberg–Teller interactions

2001

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The resonant secondary emission of light by impurity centres in crystals was studied, based on the Kramers and Heisenberg dispersion equation in time representation. The problem of the classification of the secondary emission is overviewed for an archetype model of a molecular centre. It is demonstrated that the Kramers and Heisenberg equation describes the ordinary and hot luminescence and the Rayleigh and the Raman scattering. The effects of the inhomogeneous distribution of zero-phonon transitions on different components of resonant secondary emission are described.

“…where r D a a C , a D j e j a j D i Q e i Q a i , Q a i D j c ij a j and c ij D e j Q e i ω 2 2 ω 2 1 / ω 2 i ω 2 j is the Dushinsky rotation matrix 16,17 ;…”

Section: Model Of Vibronic Systems With Pseudo-local Modesmentioning

confidence: 99%

Resonant light scattering and luminescence in multimode vibronic systems: time‐dependent representation

2001

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“…In Ref. 25, the transform law was derived for these more complicated vibronic models. Here we restrict ourselves to the results (the derivation procedure can be found in the original…”

Section: Transform Laws For Complicated Vibronic Modelsmentioning

confidence: 99%

“…x [l -exp(iojt')]p(t -t') (25) where F(t) is the Fourier transform of the absorption spectrum, w j is the Raman frequency and p(t) denotes the Fourier transform of the distribution of pureelectronic levels. For a Gaussian distribution p(t) = exp(-t2AG/2) and for a Lorentzian distribution p(t) = exp( -A,.…”

Section: Transform Law For Inhomogeneously Broadened Spectramentioning

confidence: 99%

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Resonance Raman scattering of multimode systems: Fourier amplitude approach

1993

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The time-dependent description of resonance Raman scattering of multimode systems is presented and discussed. The basic quantities of the theory are the Fourier transforms of the Raman amplitudes. For a number of vibronic models they are related to the optical absorption. These relationships enable one to transform the absorption spectrum to the Raman excitation profiles. In the transform method, model parameters are needed only for the Raman mode; the multimode information is automatically included via the measured optical absorption. The method holds for an arbitrary temperature. Transform relationships are derived for the basic model of linear vibronic coupling and for more complicated models including linear non-Condon interaction, frequency shifts and mode mixing with electronic excitation, the Jahn-Teller effect and inhomogeneous broadening.

“…Raman excitation profile) can be formulated in a form that is compact and convenient for numerical calculations. 9,11 In the case of the mutual mixing of a finite number of modes and an arbitrary number of other modes, there exist exact and simple transform relations between the Fourier transforms of the Raman amplitudes and the absorption. If the quadratic vibronic coupling is weak, an approximate transform relation exists also for an arbitrary number of mixed modes.…”

Section: Introductionmentioning

confidence: 99%

Transform method in resonance Raman scattering: effect of mode mixing

Kaasik

2002

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The effect of mode mixing on resonance Raman scattering is examined on the basis of exact transform relations for the resonance Raman excitation profiles and absorption lineshape in the time domain. General transform relations are presented which hold for an arbitrary number of mixed modes. A detailed description of the excitation profiles of two mixed Raman modes is given, taking into account an arbitrary number of other modes. The dependence of the mixing parameters, change of vibrational frequencies and equilibrium positions in the excited state on the vibronic coupling parameters is found. It is shown that in the case of a substantial change in chemical bonds at the electronic transition, the mode mixing drastically changes the Raman cross-sections/excitation profiles.